Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

doi:10.1039/C9RA04804A

Title: Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Abstract

Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.

Authors:

Wasalathanthri, Niluka D. ^[1]; Guild, Curtis ^[1]; Nizami, Quddus A. ^[2]; Dissanayake, Shanka L. ^[1]; He, Junkai ^[3]; Kerns, Peter ^[1]; Fee, Jared ^[1]; Achola, Laura ^[1]; Rathnayake, Dinithi ^[1]; Weerakkody, Chandima ^[1];

^[4]; Nandi, Partha ^[2]

Department of Chemistry, University of Connecticut, Storrs, USA
Corporate Strategic Research, ExxonMobil Research and Engineering Company, Annandale, USA
Institute of Material Science, University of Connecticut, Storrs, USA
Department of Chemistry, University of Connecticut, Storrs, USA, Institute of Material Science

Publication Date:: 2019-10-14

Research Org.:: Univ. of Connecticut, Storrs, CT (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

OSTI Identifier:: 1574081

Alternate Identifier(s):: OSTI ID: 1598224

Grant/Contract Number:: FG02-86ER13622

Resource Type:: Published Article

Journal Name:: RSC Advances

Additional Journal Information:: Journal Name: RSC Advances Journal Volume: 9 Journal Issue: 56; Journal ID: ISSN 2046-2069

Publisher:: Royal Society of Chemistry

Country of Publication:: United Kingdom

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane.  United Kingdom: N. p., 2019. 
        Web.  doi:10.1039/C9RA04804A.

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                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., & Nandi, Partha. Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane.  United Kingdom.  doi:10.1039/C9RA04804A.

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                    Wasalathanthri, Niluka D., Guild, Curtis, Nizami, Quddus A., Dissanayake, Shanka L., He, Junkai, Kerns, Peter, Fee, Jared, Achola, Laura, Rathnayake, Dinithi, Weerakkody, Chandima, Suib, Steven L., and Nandi, Partha. Mon .  
        "Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane".  United Kingdom.  doi:10.1039/C9RA04804A.

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@article{osti_1574081,

  title        = {Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane},

  author       = {Wasalathanthri, Niluka D. and Guild, Curtis and Nizami, Quddus A. and Dissanayake, Shanka L. and He, Junkai and Kerns, Peter and Fee, Jared and Achola, Laura and Rathnayake, Dinithi and Weerakkody, Chandima and Suib, Steven L. and Nandi, Partha},

  abstractNote = {Octahedral molecular sieve (OMS-2) refers to a one-dimensional 2 × 2 framework of octahedral manganese oxo units based on the cryptomelane-type framework. Herein, we describe a niobium (Nb) substituted mixed metal oxide of Nb and Mn where the cryptomelane-type framework is retained. These materials are hydrothermally synthesized from the reaction of potassium permanganate, manganese sulfate, and homogeneous niobium(V) precursors. Niobium incorporation up to 31 mol% can be achieved without destroying the one dimensional 2 × 2 framework. The yields of the materials vary between 70 and 90%. These materials are analyzed by powder XRD, BET isotherm, TEM, SEM, XRF, and XPS studies. The synthesized materials show promising activity in selective oxidation of methanol to dimethoxymethane (DMM) at 200 °C. Normalized activity correlations followed the trend 21% Nb-OMS-2 > 15% Nb-OMS-2 > 31% Nb-OMS-2 > 68% Nb-OMS-2 > K-OMS-2. A fluctuation in methanol conversion was observed around 125–150 °C in most samples, suggesting this to be a catalytically important temperature regime when forming active sites for DMM production.},

  doi          = {10.1039/C9RA04804A},

  journal      = {RSC Advances},

  number       = 56,

  volume       = 9,

  place        = {United Kingdom},

  year         = {2019},

  month        = {10}

}

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Title: Niobium-substituted octahedral molecular sieve (OMS-2) materials in selective oxidation of methanol to dimethoxymethane

Abstract

Citation Formats

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Study of the Partial Oxidation of Methanol to Formaldehyde on a Polycrystalline Ag Foil journal, June 2001

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